Proceedings of International Conference on Hybrid and Organic Photovoltaics (HOPV23)
DOI: https://doi.org/10.29363/nanoge.hopv.2023.076
Publication date: 30th March 2023
Hot-carrier solar cells are a promising candidate to exceed the detailed balance limit of 33%. One key requirement of the active material in this technology is that the cooling of hot carriers is in the order of nanoseconds to enable charge extraction. Metal halide perovskites are a promising candidate for hot-carrier materials as they show exceptionally slow cooling, often attributed to a hot-phonon bottleneck. A breakthrough was made with FASnI3 (FA being formamidinium) that shows hot-carrier emission on the nanosecond time scale.[1] However, it is unknown how the Sn-based composition affects the carrier cooling time and how the phonon lifetime is correlated with the observed hot-phonon bottleneck. In this work, we exchange FA with Cs and show that both materials show a blueshift and asymmetric broadening of the photoluminescence with increasing laser fluence, indicative of hot-carrier photoluminescence. Interestingly, the carriers in the hybrid compound cool in approximately 3 ns, much slower than sub-nanosecond cooling in the Cs system, suggesting that the organic cations play a crucial role in the cooling dynamics. By doing impulsive stimulated Raman scattering spectroscopy, we identify two coherent phonon modes (25 and 133 cm-1) in FASnI3. The 133 cm-1 mode shows a fast decay (< 1 ps) either by increasing excitation fluence or photon energy. We further show that the phonons in FASnI3 decay much faster compared to CsSnI3. These measurements correlate the pronounced hot-phonon bottleneck in hybrid compounds to the short lifetime of phonons and provide new insights into the cooling dynamics, highly relevant for the further development of hot-carrier materials.
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